Redirecting the cyclization steps of fungal polyketide synthase.

Redirecting the cyclization steps of fungal polyketide synthase. Research Abstract Details 

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Redirecting the cyclization steps of fungal polyketide synthase. Abstract Text:

Suzanne M Ma,Jixun Zhan,Xinkai Xie,Kenji Watanabe,Yi Tang,Wenjun Zhang,Suzanne M Ma,Jixun Zhan,Xinkai Xie,Kenji Watanabe,Yi Tang,Wenjun Zhang,Suzanne M Ma,Jixun Zhan,Xinkai Xie,Kenji Watanabe,Yi Tang,Wenjun Zhang,

Regiospecific cyclizations of the nascent poly-beta-ketone backbones dictate the structures of polyketide natural products. The fungal iterative megasynthases use terminal thioesterase/claisen cyclase (TE/CLC) domains to direct the fate of the polyketide chains. In this work, we present two strategies toward redirecting the cyclization steps of fungal PKSs using the Gibberella fujikuroi PKS4. First, inactivation or removal of the TE/CLC domain resulted in the synthesis of the new polyketide SMA93 2. Complementation of the mutant PKS4 with a standalone TE/CLC domain restored the regioselective cyclization steps of PKS4 and led to the synthesis of SMA76 1, demonstrating that cyclization enzymes can interact with the megasynthase in trans. This led to the second approach in which various dissociated, bacterial tailoring enzymes were added to the megasynthase in trans. Addition of the act KR led to the synthesis of mutactin 3, while the addition of first ring and second ring cyclases yielded anthraquinone compounds DMAC 5 and SEK26 6. The cooperative activities of fungal and bacterial PKS components are especially important and enable synthesis of polyketides utilizing enzymes from two distinct families of PKSs.

Redirecting the cyclization steps of fungal polyketide synthase. Publishing Authors By Initials

SM Ma,J Zhan,X Xie,K Watanabe,Y Tang,W Zhang,SM Ma,J Zhan,X Xie,K Watanabe,Y Tang,W Zhang,SM Ma,J Zhan,X Xie,K Watanabe,Y Tang,W Zhang,

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Redirecting the cyclization steps of fungal polyketide synthase. Journal Published:

PUBLICATION TYPE: Journal Article

Journal: Journal of the American Chemical Society

VOLUME: 130

Page Numbers: 38-9

Journal Abbreviation: J. Am. Chem. Soc.

ISSN: 1520-5126

DAY: 12

MONTH: 12

YEAR: 2007

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LANGUAGE: eng

NlmUniqueID: 7503056

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Grant and Affiliation Information for Redirecting the cyclization steps of fungal polyketide synthase.

AFFILIATION: Department of Chemical and Biomolecular Engineering, University of California, Los Angeles, California 90095, and Department of Pharmaceutical Sciences, School of Pharmacy, University of Southern California, Los Angeles, California 90089.

Country: United States

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MEDLINETA: J Am Chem Soc

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